Abstract
A robust method has been developed for simultaneous determination of mercury and butyltin compounds in aqueous samples. This method is capable of providing accurate results for analyte concentrations in the picogram per liter to nanogram per liter range. The simultaneous determination of the mercury and tin compounds is achieved by species-specific isotope dilution, derivatization, and gas chromatography–inductively coupled plasma mass spectrometer (GC–ICP–MS). In derivatization by ethylation and propylation, reaction conditions such as pH and the effect of chloride were carefully studied. Ethylation was found to be more sensitive to matrix effects, especially for mercury compounds. Propylation was thus the preferred derivatization method for simultaneous determination of organomercury and organotin compounds in environmental samples. The analytical method is highly accurate and precise, with RSD values of 1 and 3% for analyte concentrations in the picogram per liter to nanogram per liter range. By use of cleaning procedures and SIDMS blank measurements, detection limits in the range 10–60 pg L−1 were achieved; these are suitable for determination of background levels of these contaminants in environmental samples. This was demonstrated by using the method for analysis of real snow and seawater samples. This work illustrates the great advantage of species-specific isotope dilution for the validation of an analytical speciation method—the possibility of overcoming species transformations and non-quantitative recovery. Analysis time is saved by use of the simultaneous method, because of the use of a single sample-preparation procedure and one analysis.
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References
Craig PJ (1986) (eds) In: Organometallic compounds of environmental sciences. Principles and reactions. Longman, Essex UK
Hoch M (2001) Appl Geochem 16:719–743
Stein ED, Cohen Y, Winer AM (1996) Crit Rev Environ Sci Technol 26(1):1–43
Bouyssiere B, Szpunar J, Lobinski R (2002) Spectrochim Acta Part B 57:805–828
Moens L, De Smaele T, Dams R, Van Den Broeck P, Sandra P (1997) Anal Chem 69:1604–1611
Prange A, Jantzen E (1995) J Anal At Spectrom 10:15–109
De Smaele T, Moens L, Dams R, Sandra P (1996) Fresenius J Anal Chem 355:778–782
Ruiz Encinar J, Rodiguez Gonzales P, Garcia Alonso JI, Sanz Medel A (2003) Trends Anal Chem 22(2):108–114
Rodriguez Martin Doimeadios R, Monperrus M, Krupp E, Amouroux D, Donard OFX (2004) Trends Anal Chem 23(3):261–272
Rapsomanikis S (1994) Analyst 119:1429–1439
De Smaele T, Moens L, Dams R, Sandra P, Van Der Eycken J, Vandyck J (1998) J Chromatogr A 793:99–106
Schubert P, Rosenberg E, Grasserbauer M (2000) Fresenius J Anal Chem 366:356–360
Demuth N, Heumann KG (2001) Anal Chem 73:4020–4027
Grinberg P, Campos RC, Mester Z, Sturgeon RE (2003) J Anal At Spectrom 18:902–909
Ruiz Encinar J, Rodriguez Gonzales P, Garcia Alonso JI, Sanz Medel A (2002) Anal Chem 74:270–281
Rodriguez Martin Doimeadios RC, Monperrus M, Krupp E, Amouroux D, Donard OFX (2003) Anal Chem 75:3202–3211
Rodriguez Martin doimeadios R, Krupp E, Amouroux D, Donard OFX (2002) Anal Chem 74:2505–2512
Hintelmann H, Evans RD (1997) Fresenius J Anal Chem 358:378–385
Heumann KG, Gallus SM, Radlinger G, Volg L (1998) Spectrochim Acta Part B 53:273–287
Yang L, Mester Z, Sturgeon RE (2003) J Anal At Spectrom 18:431–436
Monperrus M, Rodriguez Martin Doimeadois RC, Scancar J, Amouroux D, Donard OFX (2003) Anal Chem 75:4095–4102
Gelaude L, Dams R, Resano M, VanHaecke F, Moens L (2002) Anal Chem 74:3833–3842
Yang L, Mester Z, sturgeon R (2002) Anal Chem 74:2968–2976
Ruiz Encinar J, Garcia Alonso JI, Sanz Medel A (2000) J Anal At Spectrom 15:1233–1239
Snell JP, Stewart IL, Sturgeon RE, Frech W (2000) J Anal At Spectrom 15:1540–1545
Monperrus M, Zuloaga O, Krupp E, Amouroux D, Whalen R, Fairman B, Donard OFX (2003) J Anal At Spectrom 18:247–253
Kingston HM, Huo D, Luo Y, Chalk S (1998) Spectrochim Acta Part B 53:299–309
Sutton PG, Harrington CF, Fairman B, Evans EH, Ebdon L, Catterick T (2000) Appl Organomet Chem 14:391–700
Rodriguez Martin Doimeadios RC, Stoickev T, Krupp E, Amouroux D, Holeman M, Donard OFX (2002) Appl Organomet Chem 16:610–615
De Diego A, Tseng CM, Stoickev, Amouroux D, Donard OFX (1998) J Anal At Spectrom 13:623–629
Carpinteiro Botana J, Rodil Rodriguez R, Carro Diaz AM, Lorenzo Ferreira RA, Cela Torrijos R, Rodriguez Pereiro I (2002) J Anal At Spectrom 17:904–907
Inaba K, Shiraishi H, Soma Y (1995) Water Res 29(5):1415–1417
Acknowledgements
The authors would like to thank Thermo Elemental for providing the X7 series ICP–MS and focus GC, which were used throughout this study. M.M. acknowledges the Conseil général des Pyrénées Atlantiques for her Ph.D. financial support. E.T. acknowledges INERIS for his financial support. S. Veschambre is thanked for sampling snow samples.
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Monperrus, M., Tessier, E., Veschambre, S. et al. Simultaneous speciation of mercury and butyltin compounds in natural waters and snow by propylation and species-specific isotope dilution mass spectrometry analysis. Anal Bioanal Chem 381, 854–862 (2005). https://doi.org/10.1007/s00216-004-2973-7
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DOI: https://doi.org/10.1007/s00216-004-2973-7